Growth of Au Hollow Stars and Harmonic Excitation Energy Transfer

Optical excitation, subsequent energy transfer, and emission are fundamental to many physical problems. Optical antennas are ideal candidates for manipulating these processes. We extend energy transfer to second- and third-harmonic (SH and TH) fields through the collaborative susceptibility χ⁽ (n = 1, 2, 3) resonances of nonlinear optical antennas. Hollow gold stars, with a broadband response covering the fundamental, SH, and TH frequencies, are synthesized as nonlinear antennas. Harmonic resonance energy transfer through a χ⁽³⁾ → χ⁽¹⁾ collaboration is revealed. A χ⁽³⁾ → χ⁽²⁾ collaboration is uncovered, with largely enhanced SH radiation demonstrated by exciting the three resonances at the fundamental, SH, and TH frequencies. A theoretical model of the effective nonlinear susceptibilities is proposed to calculate the efficiencies of the two nonlinear energy transfer processes.